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Electrified inductive heating for sustainable utilization of liquid hydrogenated organics 电感应加热促进液态氢化有机物的可持续利用
IF 38.6 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-08-21 DOI: 10.1016/j.joule.2024.05.020

We propose the electrified catalytic inductive heating system (ECIHS), which utilizes electromagnetic induction heating (IH) of a monolithic catalytic composite to induce direct and efficient heat transfer to the liquid-phase reaction environment. Herein, we demonstrated that the ECIHS could be utilized to extract hydrogen from liquid-phase perhydro-dibenzyltoluene (H18-DBT) within just 3.5 s, accounting for a 16.4-fold improvement in the reaction rate compared with conventional heating methods. This remarkable observation underscores the potential of the ECIHS for on-site hydrogen utilization, empowering various advanced applications such as hydrogen-powered vehicles. Furthermore, the capabilities of the ECIHS for efficient heat and mass transfer in the liquid phase are also translatable to a myriad of different chemical processing schemes with high industrial value. Overall, the ECIHS represents a major breakthrough in the development of sustainable chemical processing methods, further propelling efforts to achieve full decarbonization in the global chemical processing industry.

我们提出了电气化催化感应加热系统(ECIHS),该系统利用电磁感应加热(IH)整体催化复合材料,将热量直接有效地传递到液相反应环境中。在这里,我们证明了 ECIHS 可用于在短短 3.5 秒内从液相全氢二苄甲苯(H18-DBT)中提取氢气,与传统加热方法相比,反应速率提高了 16.4 倍。这一引人注目的观察结果凸显了 ECIHS 在现场氢气利用方面的潜力,为氢动力汽车等各种先进应用提供了动力。此外,ECIHS 在液相中高效传热和传质的能力还可应用于各种不同的化学处理方案,具有极高的工业价值。总之,ECIHS 代表着可持续化学处理方法开发方面的重大突破,进一步推动了全球化学处理行业实现全面脱碳的努力。
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引用次数: 0
Mechanically durable chiral-structured heterointerfaces 具有机械耐久性的手性结构异质界面
IF 38.6 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-08-21 DOI: 10.1016/j.joule.2024.07.014
Jin-Wook Lee

While interface engineering of perovskite solar cells (PSCs) for defect passivation and band alignment optimization has contributed to recent breakthroughs in the efficiency and stability of PSCs, consideration of the mechanical reliability of the heterointerface has been relatively overlooked. Published in Science, the study by Duan et al.1 proposes that chiral-structured heterointerfaces are mechanically more durable compared to the widely used non-chiral heterointerfaces in PSCs.

虽然用于缺陷钝化和带排列优化的过氧化物太阳能电池(PSCs)界面工程有助于最近在 PSCs 的效率和稳定性方面取得突破,但对异质界面的机械可靠性的考虑却相对被忽视了。Duan 等人1 发表在《科学》杂志上的研究提出,与 PSC 中广泛使用的非手性异质界面相比,手性结构异质界面的机械耐久性更高。
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引用次数: 0
General design of high-performance and textured layered thermoelectric materials via stacking of mechanically exfoliated crystals 通过机械剥离晶体堆叠实现高性能纹理层状热电材料的总体设计
IF 38.6 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-08-21 DOI: 10.1016/j.joule.2024.05.006

Layered materials exhibit potential for thermoelectric applications, which are reliant on microstructural texture for high performance. In this work, we present layered crystal stacking hot deformation (LCSHD), which leverages anisotropic crystal structures to induce rapid texture formation, leading to high thermoelectric performance. Taking n-type bismuth telluride (Bi2Te3) as a representative, the LCSHD method contributed to a record-high power factor (PF) of 45 μW cm−1 K−2 in polycrystals. Additionally, the dislocation tangle and low-angle grain boundary can be found in the LCSHD sample, producing low lattice thermal conductivity and a remarkable ZT value of 1.2. Benefiting from a reliable high ZT, we prepared a seven-pair Bi2Te3-based module, which displayed an extraordinary conversion efficiency of 6.4% and competitive refrigeration performance. In addition, a significant improvement of ZT value in other layered materials, including SnSe2 and SnSe, was also demonstrated. Our finding offers novel avenues for texture engineering, facilitating the design of high-performance layered thermoelectric materials.

层状材料具有热电应用的潜力,而热电应用的高性能依赖于微结构纹理。在这项工作中,我们提出了层状晶体堆叠热变形(LCSHD),它利用各向异性晶体结构诱导纹理的快速形成,从而实现高热电性能。以 n 型碲化铋(Bi2Te3)为代表,LCSHD 方法使多晶体的功率因数(PF)达到了创纪录的 45 μW cm-1 K-2。此外,在 LCSHD 样品中还发现了位错纠结和低角度晶界,从而产生了低晶格热导率和 1.2 的显著 ZT 值。得益于可靠的高 ZT 值,我们制备出了基于 Bi2Te3 的七对模块,其转换效率高达 6.4%,制冷性能极具竞争力。此外,其他层状材料(包括 SnSe2 和 SnSe)的 ZT 值也得到了显著改善。我们的发现为质构工程提供了新的途径,有助于高性能层状热电材料的设计。
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引用次数: 0
Disorder and spin-electron interaction in oxide cathodes 氧化物阴极中的无序和自旋电子相互作用
IF 38.6 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-08-21 DOI: 10.1016/j.joule.2024.07.022
Qinghe Zhao , Feng Pan

The quest for high-performance lithium-ion batteries has led to extensive research on developing the advanced cathodes. A recent report in Nature by Wang et al. presents a strategy of integrating chemical short-range disorder into the bulk structure of layered oxide cathodes, which significantly enhances their durability and rate capability due to the subtle tuning of spin-electron interactions of transition metal ions.

对高性能锂离子电池的追求促使人们对先进阴极的开发进行了广泛的研究。Wang 等人最近在《自然》(Nature)杂志上发表的一篇报告介绍了一种将化学短程无序整合到层状氧化物阴极体结构中的策略,由于过渡金属离子自旋电子相互作用的微妙调整,这种策略显著提高了阴极的耐久性和速率能力。
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引用次数: 0
Suppressed deprotonation enables a durable buried interface in tin-lead perovskite for all-perovskite tandem solar cells 抑制去质子化使锡铅包晶石中的持久埋藏界面适用于全包晶石串联太阳能电池
IF 38.6 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-08-21 DOI: 10.1016/j.joule.2024.05.007

Low-band-gap tin (Sn)-lead (Pb) perovskites are a critical component in all-perovskite tandem solar cells (APTSCs). Current state-of-the-art Sn-Pb perovskite devices exclusively use poly(3,4-ethylenedioxythiophene)-poly(styrenesulfonate) (PEDOT:PSS) as the hole-transport layer (HTL) but suffer from undesired buried-interface degradation. Here, we show that the deprotonation of the –SO3H group in PSS is the root cause of the interface degradation due to its low acid dissociation constant (pKa), leading to acidic erosion and iodine volatilization in Sn-Pb perovskites. We identify that HTL featuring the carboxyl (–COOH) group with a higher pKa, such as poly[3-(4-carboxybutyl)thiophene-2,5-diyl] (P3CT), can suppress deprotonation and strengthen the interface, mitigating the buried-interface degradation. Motivated by established P3CT modification, we introduce Pb doping to P3CT to increase its work function and reduce interfacial energy loss. We fabricate APTSCs with a champion efficiency of 27.8% and an operational lifetime of over 1,000 h, with 97% retaining efficiency under maximum power point tracking.

低带隙锡(Sn)-铅(Pb)包晶石是全包晶石串联太阳能电池(APTSC)的重要组成部分。目前最先进的锡铅包晶器件专门使用聚(3,4-亚乙二氧基噻吩)-聚(苯乙烯磺酸)(PEDOT:PSS)作为空穴传输层(HTL),但却受到埋藏界面降解的困扰。在这里,我们发现 PSS 中 -SO3H 基团的去质子化是导致界面降解的根本原因,因为它的酸解离常数 (pKa) 很低,从而导致锡铅包晶石中的酸性侵蚀和碘挥发。我们发现,具有较高 pKa 的羧基(-COOH)的 HTL(如聚[3-(4-羧基丁基)噻吩-2,5-二基](P3CT))可以抑制去质子化并强化界面,从而减轻埋藏界面降解。受已建立的 P3CT 改性技术的启发,我们在 P3CT 中掺入了铅,以增加其功函数并减少界面能量损失。我们制造的 APTSC 的冠军效率为 27.8%,工作寿命超过 1,000 小时,在最大功率点跟踪下的保持效率为 97%。
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引用次数: 0
A polymer acceptor with double-decker configuration enhances molecular packing for high-performance all-polymer solar cells 具有双层构型的聚合物受体可增强高性能全聚合物太阳能电池的分子填料性能
IF 38.6 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-08-21 DOI: 10.1016/j.joule.2024.06.010

All-polymer solar cells (all-PSCs) have seen rapid progress enabled by the development of high-performance polymer acceptors. Most polymer acceptors are based on the monomers of a classic small molecular acceptor (SMA) named Y6 by polymerizing at the position of the end groups, forming an “end-to-end” linkage. In this work, we report a completely different “core-to-core” linking mode by polymerizing the Y-series monomers at the central core position instead. This innovative strategy results in a drastically altered molecular configuration that resembles a “double decker,” with intramolecular packing between different monomer units in the same polymer. The overall molecular packing is improved, benefiting charge delocalization and charge transport. As a result, the PffBQx-T-based ternary blend achieved an outstanding efficiency of 18.7%, attributed to the enhanced absorption response, improved packing, and efficient charge dynamics. Our work demonstrates a novel polymer design rationale that serves as a promising avenue toward highly efficient and stable all-PSCs.

随着高性能聚合物受体的开发,全聚合物太阳能电池(all-PSCs)取得了突飞猛进的发展。大多数聚合物受体都是以一种名为 Y6 的经典小分子受体(SMA)的单体为基础,通过在端基位置聚合,形成 "端对端 "连接。在这项工作中,我们报告了一种完全不同的 "核对核 "连接模式,即在中心核位置聚合 Y 系列单体。这种创新策略大大改变了分子构型,使其类似于 "双层",同一聚合物中不同单体单元之间形成分子内堆积。整体分子堆积得到改善,有利于电荷分散和电荷传输。因此,基于 PffBQx-T 的三元共混物达到了 18.7% 的出色效率,这归功于增强的吸收响应、改进的堆积和高效的电荷动力学。我们的工作展示了一种新颖的聚合物设计原理,为实现高效、稳定的全聚苯乙烯多氯联苯(all-PSCs)提供了一条大有可为的途径。
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引用次数: 0
Supramolecular design principles in pseudohalides for high-performance perovskite solar mini modules 用于高性能过氧化物太阳能微型模块的伪卤化物超分子设计原理
IF 38.6 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-08-21 DOI: 10.1016/j.joule.2024.05.019

In this work, we reveal the role of non-covalent interactions, which are known to play important roles in supramolecular phenomena, in achieving efficient perovskite surface and grain boundary passivation. By using a series of pseudohalides, we find that trifluoroacetate (TFA) provides the strongest binding to iodide vacancies by means of non-covalent hydrogen bonding and dispersion interactions. By exploiting additional non-covalent dispersion and hydrophobic interactions in aromatic 3,3-diphenylpropylammonium (DPA+), we present a dual-ion passivation strategy that not only minimizes the non-radiative recombination center and local chemical inhomogeneities but also induces preferentially oriented growth of α-FAPbI3 lattice. This leads to an outstanding power conversion efficiency (PCE) of 25.63% with an exceptional open-circuit voltage of 1.191 V in a perovskite solar cell with a small area, while perovskite solar mini modules with aperture areas of 25 and 64 cm2 achieved PCE of 22.47% (quasi-steady-state [QSS]-certified 20.50%) and 20.88%, respectively, with outstanding stability under high-humidity conditions.

在这项研究中,我们揭示了在超分子现象中发挥重要作用的非共价相互作用在实现高效的包晶表面和晶界钝化中的作用。通过使用一系列伪卤化物,我们发现三氟乙酸盐(TFA-)通过非共价氢键和弥散相互作用为碘化物空位提供了最强的结合力。通过利用芳香族 3,3-二苯基丙基铵(DPA+)中额外的非共价分散和疏水相互作用,我们提出了一种双离子钝化策略,不仅能最大限度地减少非辐射重组中心和局部化学不均匀性,还能诱导 α-FAPbI3 晶格优先定向生长。这使得小面积的透辉石太阳能电池的功率转换效率(PCE)达到 25.63%,开路电压达到 1.191 V,而孔径面积分别为 25 和 64 cm2 的透辉石太阳能微型模块的 PCE 分别达到 22.47%(准稳态 [QSS] 认证为 20.50%)和 20.88%,并且在高湿度条件下具有出色的稳定性。
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引用次数: 0
Nanochannel electrodes facilitating interfacial transport for PEM water electrolysis 促进 PEM 水电解界面传输的纳米通道电极
IF 38.6 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-08-21 DOI: 10.1016/j.joule.2024.06.005

Proton-exchange membrane water electrolyzers (PEMWEs) are a promising technology for green hydrogen production; however, interfacial transport behaviors are poorly understood, hindering device performance and longevity. Here, we first utilized finite-gap electrolyzer to demonstrate the possibility of proton transfer through water in PEMWEs. The measured high-frequency resistances (HFRs) exhibit a linear trend with increasing gap distance, where extrapolation shows a lower value compared with HFRs in regular zero-gap electrolyzers, indicating that ohmic resistance could be further reduced. We introduce nanochannels to facilitate mass transport, as evidenced by both liquid-fed and vapor-fed electrolysis. Nanochannel electrodes achieve a voltage reduction of 190 mV at 9 A·cm−2 compared with the Ir-PTEs without nanochannels. Furthermore, nanochannel electrodes show negligible degradation through 100,000 accelerated-stress tests and over 2,000 h of operation at 1.8 A·cm−2 with a decay rate of 11.66 μV·h−1. These results provide new insights into localized transport dynamics for PEMWEs and highlight the significance of interfacial engineering for electrochemical devices.

质子交换膜水电解槽(PEMWEs)是一种前景广阔的绿色制氢技术;然而,人们对其界面传输行为知之甚少,从而影响了设备的性能和寿命。在这里,我们首次利用有限间隙电解槽证明了质子在 PEMWEs 中通过水传输的可能性。测得的高频电阻(HFR)随着间隙距离的增加呈线性趋势,外推法显示,与普通零间隙电解槽中的高频电阻相比,高频电阻值更低,这表明欧姆电阻可以进一步降低。我们引入了纳米通道来促进质量传输,这在液体馈电和蒸汽馈电电解中都得到了证明。与不带纳米通道的 Ir-PTE 相比,纳米通道电极在 9 A-cm-2 的电压下可降低 190 mV。此外,纳米沟道电极在 1.8 A-cm-2 下经过 100,000 次加速应力测试和超过 2,000 小时的运行后,衰减率为 11.66 μV-h-1,可以忽略不计。这些结果为 PEMWEs 的局部传输动力学提供了新的见解,并突出了界面工程对电化学设备的重要意义。
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引用次数: 0
Design of low-cost non-fused ultranarrow-band-gap acceptors for versatile photovoltaic applications 为多功能光伏应用设计低成本非熔融超宽带隙受体
IF 38.6 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-08-21 DOI: 10.1016/j.joule.2024.05.011

Ultranarrow-band-gap organic semiconductors with fully non-fused conjugated structures display great potential for low-cost organic photoelectric devices. Here, we developed two fully non-fused acceptors, namely, A4T-7 and A4T-12, by introducing different alkoxyl side chains on the π-bridges of the non-fused acceptors. The resulting materials demonstrate ultranarrow optical band gaps of 1.15 and 1.21 eV, respectively. Compared with other ultranarrow-band-gap acceptors constructed with fully fused-ring or partially fused-ring structures, the synthetic complexity of the two acceptors is significantly reduced. Specifically, A4T-7, with symmetric alkoxy chains on the π-bridge, exhibits a more planar molecular configuration compared with A4T-12. Notably, the organic photovoltaic cells based on A4T-7 show a power conversion efficiency of 13.3%. Moreover, cells fabricated with a highly transparent active layer, characterized by an average visible transmittance value of approximately 62.7%, achieve an efficiency of 10.7%. These results represent the highest reported efficiencies for cells utilizing fully non-fused acceptors with ultranarrow band gaps.

具有完全非融合共轭结构的超宽带隙有机半导体在低成本有机光电器件方面具有巨大潜力。在这里,我们通过在非融合受体的 π 桥上引入不同的烷氧基侧链,开发出了两种完全非融合受体,即 A4T-7 和 A4T-12。这两种材料的超窄光带隙分别为 1.15 和 1.21 eV。与其他完全熔环或部分熔环结构的超宽带隙受体相比,这两种受体的合成复杂性大大降低。具体来说,与 A4T-12 相比,π 桥上带有对称烷氧基链的 A4T-7 显示出更平面的分子构型。值得注意的是,基于 A4T-7 的有机光伏电池的功率转换效率高达 13.3%。此外,使用高透明活性层制造的电池(平均可见光透射率约为 62.7%)的效率也达到了 10.7%。这些结果代表了利用具有超窄带隙的完全非熔化受体的电池的最高效率。
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引用次数: 0
Perfluoroalkylsulfonyl ammonium for humidity- resistant printing high-performance phase-pure FAPbI3 perovskite solar cells and modules 用于耐湿印刷高性能相纯 FAPbI3 包晶太阳能电池和模块的全氟烷基磺酰铵
IF 38.6 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-08-21 DOI: 10.1016/j.joule.2024.05.018

High-quality phase-pure formamidinium lead triiodide (FAPbI3) perovskite film needs to be fabricated under strict control of the surrounding atmosphere, which becomes more rigorous when large-area FAPbI3 film is involved, leading to high-performance FAPbI3 perovskite solar cells and modules predominantly carried out in an inert gas-filled atmosphere. In this work, we propose a scalable printing strategy for the large-area high-quality phase-pure FAPbI3 film under a high-humidity atmosphere (up to 75% ± 5% relative humidity) by regulating the perovskite precursor ink with a functional perfluoroalkylsulfonyl quaternary ammonium iodide. This approach decreases the energy barriers of cubic phase formation and heterogeneous nucleation, thereby regulating the FAPbI3 crystallization. The printed photovoltaic small-area cells and large-area modules achieved remarkable power conversion efficiencies of 24.37% and 22.00%, respectively. Specifically, the unencapsulated device exhibits superior operational stability with T90 > 1,060 h, ambient stability with T90 > 2,020 h, and thermal stability with T90 > 2,350 h.

高质量相纯三碘化甲脒铅 (FAPbI3) 包晶石薄膜需要在严格控制周围气氛的条件下制造,当涉及大面积 FAPbI3 薄膜时,这种控制变得更加严格,从而导致高性能 FAPbI3 包晶石太阳能电池和模块主要在充满惰性气体的气氛中进行。在这项工作中,我们提出了一种在高湿度环境(相对湿度高达 75% ± 5%)下大面积生产高质量相纯 FAPbI3 薄膜的可扩展印刷策略,方法是用功能性全氟烷基磺酰基季铵碘化物调节包晶石前驱体油墨。这种方法降低了立方相形成和异质成核的能量障碍,从而调节了 FAPbI3 的结晶。印刷光伏小面积电池和大面积模块的功率转换效率分别达到了 24.37% 和 22.00%。具体而言,未封装器件在 T90 > 1,060 小时内表现出卓越的工作稳定性,在 T90 > 2,020 小时内表现出卓越的环境稳定性,在 T90 > 2,350 小时内表现出卓越的热稳定性。
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引用次数: 0
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